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JournalofHazardousMaterials
journalhomepage:
ResearchPaper
SuperiorremovalofAs(III)andAs(V)fromwaterwithMn-dopedβ-FeOOH
nanospindlesoncarbonfoam
BingYana,c,*,TianLiangb,XiaohuiYangb,,**
aSchoolofEnvironmentalStudies,ChinaUniversityofGeosciences,Wuhan430074,PRChina
bFacultyofMaterialsScienceandChemistry,ChinaUniversityofGeosciences,Wuhan430074,PRChina
cDepartmentofCivilandEnvironmentalEngineering,UniversityofCalifornia,Berkeley,CA94720-1710,USA
ARTICLEINFOABSTRACT
Editor:-based
,theygenerallysufferfromlow
Keywords:removalefficiencytowardshighlytoxicAs(III),lossofactivesitesowingtoagglomeration,andpoorreusability.
ArsenicremovalHerein,wereportacarbonizedmelaminefoamsupportedMn(IV)-dopedβ-FeOOHnanospindles(******@Mn-FeOOH
MonolithNSp)fortacklingthetechnicalhurdles.******@Mn-FeOOHNSpappearsasafree-standingmonolith
Manganesedoping
throughalow--scaleintegrationofMn(IV)into
FeOOH
β-FeOOHenablesanoxidation-adsorptionbifunctionality,whereMn(IV)servesasoxidizerforAs(III)andFe(III)
Oxidation-adsorption
actsasadsorberforAs(V).ThemaximaladsorptioncapacityforAs(V)andAs(III)canreach152and107mgg1,
,Asinsimulatedhigharsenicgroundwatercanbedecreasedtobelow10μgL1within
“filtrating-washing”,85%and82%ofitsinitialadsorptioncapacityforAs(V)andAs(III)canbe
easilyrecoveredevenafter5-
adsorptionbehaviorismainlythroughchemicalbondingduringsingle--prepared
******@Mn-FeOOHoffersascalable,efficient,andrecyclablesolutionforarsenicremovalingroundwaterand
wastewaterfromminesandindustry.
(Wongetal.,2017),isconsideredasoneofthe
Themaximumcontaminantlimitofarsenicindrinkingwaterpro­arsenicinwaterforitsexcellentadsorptioncapacitytowardsarsenate
posedbyWorldHealthOrganization(WHO-MCL)is10μgL1(Muthu(As(V))(Fuetal.,2017;Pengetal.,2013;Zhangetal.,2007).However,
Prabhuetal.,2019;Jainetal.,2009).However,higharseniccontami­FeOOHhaslimitedabilitytoremovearsenite(As(III)),whichis60times
nationofgroundwaterusedfordrinkingiswidelydistributedworldwidetoxicityhigherthanAs(V)(Fengetal.,2012;ShanandTong,2013).
(Rodriguez-Ladoetal.,2013;Habuda-StanicandNujic,2015).TheThus,externaloxidantsareoftenutilizedtotransformAs(III)to
inappropriatedisposalofarsenicwastewaterfromminesandindustryless-toxicAs(V)forsubsequentcaptureandremovalbyFeOOHin
(usuallyatconcentrationsoftensofmgL1andmainlyasAs(III))(III)isthepredominantAsspeciesinmanyareasof
continuestocontaminatethedrinkingwater(Egaletal.,2009;Ahorantahigharsenicgroundwater(LienandWilkin,2005;Sorgetal.,2014),
etal.,2016).Therefore,itisextremelyimportantandurgenttodevelopaddingoxidantsingroundwaterremediationwillinevitablychangethe
(VogelinandHug,
Numeroustechnologies,includingadsorption(Yanetal.,2016),2003).Therefore,tosynthesizeiron-manganesebinaryoxidewithdual
coagulation-precipitation(Matsuietal.,2017),biologicaldegradationfunctionof“oxidation-adsorption”isusuallyadoptedtosolvethis
(Tianetal.,2012;Linetal.,2018),andionexchange(Ortegaetal.,problem,whereMnplaysasanintrinsicoxidanttooxidizeAs(III)toAs
2017),(V)(ShanandTong,2013;McCannetal.,2018;Zhangetal.,2012;
owingtoitseaseofoperation,low-cost,hightreatmentefficiency,andZhangetal.,2007),whichcanbemorereadilyadsorbedonthe
*Correspondingauthorat:SchoolofEnvironmentalStudies,ChinaUniversityofGeosciences,Wuhan430074,PRChina.
**Correspondingauthor.
E-mailaddresses:******@(),******@().
/
Received22March2021;Receivedinrevisedform23May2021;Accepted4June2021
Availableonline7June2021
0304-3894/©.
(2021)126347
.
-situprocessavoidsthesecondarypollutionpreparedaccordingtotheaboveprocedureswithoutMnCl24H2O.
,Mn,Fe,andO
cannotbedistributedevenlyiniron-
preparedviatraditionalmethods(physicalmixingorco-precipitation),
whichleadstopartialshieldingbetweenactivesitesandresultsinThecrystallinemineralcompositionwasmeasuredbyX-ray
inferiorarsenicremovalperformance(Tresintsietal.,2013).diffraction(XRD,BrukerD8-FOCUSpowderdiffractionsystem).A
Atomic-scaledopingofMn(IV)intotheFOOHlatticecaneffectivelyFouriertransforminfrared(FTIR)spectrometer(NicoletiS50)inthe
exposeactivesitesandfacilitatethein-situ“oxidation-adsorption”,rangeof400–4000cm1bymeansoftheKBrpellettechniquewasused
contributingtoahighperformanceofAsadsorption(Tresintsietal.,
2013;Pinakidouetal.,2016).Inlightofthis,ahydrothermalprepara­byaZetapotentialanalyzer(NanoZS90,UK).ThermoFisherESCALAB
tionofMn-dopedβ-FeOOH(Mn-FeOOH)-rayphotoelectronspectroscopy(XPS).The
atomic-scaledopingcanconstructasingle-phaseMn(IV)-FeOOHnano­morphologyandnanostructureoftheobtainedsampleswereexamined
spindles,whichpromotesthehomogeneousdistributionofthedualusingfield-emissionscanningelectronmicroscope(FE-SEM,Hitachi
activecenterof"oxidationMn(IV)-adsorptionFe(III)",).TheBrunauer-Emmett-Teller(BET)specificsurface
,consideringtheareawasmeasuredusingMicromeriticsASAP2046Analyzer,whilethe
commondrawbacksofagglomerationandrecyclingdifficultyasnano­poresizedistributionsofthesampleswerecalculatedbyadoptingthe
material,themacroscopicporousscaffoldofoxidizedcarbonfoamareBarrett-Joyner-Halenda(BJH)model.
adoptedtosupportnano-adsorbentofMn(IV)-FeOOHnanospindles,
whichenablesthecompositetoberecycledeasilythroughafacile“fil­
trating-washing”process,overcomingthedrawbackofconventional
powderedMn(IV)-FeOOHnanomaterial(Geetal.,2017).Besides,theBatchadsorptionexperimentswereperformedatfixedtemperature
◦
carbonfoamisderivedfromthemelaminefoam(MF),whichisakindofof25C,,
commercialpolymerthathaslowcost,highflexibility,andlarge-scalereactiontime,initialconcentrationofarsenicandco-existingcompeting
,theporousstructureofthescaffoldpro­anionsonarsenicremovalinsyntheticAs(V)andAs(III)solution
videsplentifulchannelsforthemasstransportationofAs(III)
dual-centers(oxidationMn(IV)-adsorptionFe(III)),enhancingthedilutedHClandNaOHsolution().
Inthisstudy,weproposethehydrothermalpreparationofafree-arsenicadsorptioncapacitiesofadsorbentsinAs(V)andAs(III)solution
standingcompositeofMn-FeOOHassembledonoxidizedcarbonfoamwithinitialconcentrationsrangedfrom1to500mgL1atpH=
(******@Mn-FeOOH),whichexhibitsexcellentadsorbingcapacitytowardsadsorptionkineticswerestudiedatpH=7for24hin20mLof10mgL1
bothAs(V)andAs(III).,itcanreduceAs(III)eitherAs(V)orAs(III)
andAs(V)from1mgL1tobelow10μgL1(WHO-MCL)within24harsenicremoval,
and12h,respectively,exceedingthemostcommoniron-basedadsor­solutions(with20mgL1ofeitherAs(III)orAs(V))for24hwith
bents(Fengetal.,2012;ShanandTong,2013;McCannetal.,2018;differentinitialpH,whichwereadjustedto2,4,6,7,8and10respec­
Zhangetal.,2012,2007,2013;Tresintsietal.,2013;Changetal.,2009;-existingcompetinganionsasCl-(NaCl,
-2-3-
Chenetal.,2013;GuptaandGhosh,2009;ShevadeandFord,2004;%),HCO3(NaHCO3,>99%),SO4(Na2SO4⋅10H2O,>99%)andPO4
etal.,2012;Andjelkovicetal.,2015).Therawmaterialsusedforpre­(NaH2PO4,%)onarsenicadsorptionwereinvestigatedattwoion
paringthecompositeareallinexpensiveandreadilyavailable($12kg1concentrations()in10mgL1ofeitherAs(V)orAs
forMF),alongwiththestraightforwardpreparingmethodandefficient(III)solution.
arsenicadsorptionperformance,******@Mn-FeOOHtobeaThehighconcentrationsofsolubleAs(>1mgL1)weremeasured
(ICP-
AES),whilethelowconcentrations(<1mgL1)weredeterminedby
(AFS).AqueousAs(V)andAs(III)
wereseparatedbyfilteringthefiltratewithAs-speciationanionex­
(,1998;Guoetal.,2008)beforetesting.
Allchemicalsusedinthisstudywereofanalyticalgrade(-******@Mn-FeOOHstudy
ChemicalReagentCo.,Ltd.,China).Arsenicsolutionswerepreparedby
dissolvingNa2HAsO4andNaAsO2indeionizedwater,-OOH,andunravelthe
wasprovidedbyKelinmeiCompanyinChina.‘oxidation-adsorption’mechanismoftheadsorbent,******@Mn-FeOOH
******@FeOOHwerecomparedintheabovebatchexperiments
.******@Mn-,lowerconcentrationofAs(III)andAs(V)
(1mgL1),similartogeogenichigharsenicgroundwater,wereadopted
Carbonfoam(CF)wasderivedfrommelaminefoam(MF)
◦
carbonizationunderN2(at700Cfor2h,******@Mn-FeOOH,Asspeciationin
◦
5Cmin1),andcuttedintoslabs(3××).TheCFpiecesweretheresidualsolutionwasseparatedtoAs(III)andAs(V)beforeAFS
1◦
thenacidizedby3molLH2SO4andheatedat120Cfor1hrespec­analysis(Yanetal.,2002).
◦
,theslabswerewashedanddried(T=50C)toacquire
Mn-FeOOHnanospindleswasobtainedbyhydrothermalprocessin
..
(),-obtainedmaterialsforarsenic
(,5%oftheironmolarratio),32mmolNaNO3(),,theadsorbentwassubjectedtoafive-cycleadsorption-
HCl(%),
1
(C2H3N,>99%).(V)orAs(III)solution.
◦
andstirredforanother60minandheatedat100Cfor4htoprepareAftereachadsorptioncycle,theadsorbentwasfiltered,washedwith
******@Mn-FeOOHNSp.******@FeOOHNSpswasseparatelyNaOHsolution()for30min,thenrinsedwithdeionized
2
(2021)126347
1
water,soakedinH2SO4solution()for10min,followedbybaxiswouldbecompressed,whilethecaxiswasstretched(TableS1,
).TheXRDresultsdemonstratethesinglephase
ofMndopedFeOOHandimplytheuniformdistributionofMnon
.
BETandBJHanalyseswereemployedtoanalyzethespecificsurface
­
,MFturnedfromwhitetoblack,withits(b)and(c).TheBETspecificsurfaceareaofthesamples(TableS2,
%,owingtothethermalSupportingInformation)illustratesthatthespecificsurfaceareaswere
­asfollowed:Mn-FeOOH()>FeOOH()
phobic,anacidpre-oxidationwasfurthercarriedouttoincreasethe>******@Mn-FeOOH()>******@FeOOH()>CF